共压共烧法制备La0.8Sr0.2(Ga0.8Mg0.2)0.1Fe0.9O3-δ致密扩散障碍层极限电流型氧传感器

doi:10.15541/jim20160693

无机材料学报 ›› 2017, Vol. 32 ›› Issue (10): 1089-1094.DOI: 10.15541/jim20160693 CSTR: 32189.14.10.15541/jim20160693

共压共烧法制备La_0.8Sr_0.2(Ga_0.8Mg_0.2)_0.1Fe_0.9O_3-_δ致密扩散障碍层极限电流型氧传感器

张小芳, 刘涛, 金宏斌, 于景坤, 高翔, 王成, 王相南

(东北大学冶金学院, 沈阳 110819)

收稿日期:2016-12-22 修回日期:2017-02-23 出版日期:2017-10-20 网络出版日期:2017-09-21
作者简介:张小芳(1983–), 女, 博士研究生. E-mail: xfzhang2009@163.com
基金资助:
国家自然科学基金(51374055;52174059)

La_0.8Sr_0.2(Ga_0.8Mg_0.2)_0.1Fe_0.9O_3-_δ Dense Diffusion Barrier Limiting Current Oxygen Sensor Prepared by Co-pressing and Co-sintering Method

ZHANG Xiao-Fang, LIU Tao, JIN Hong-Bin, YU Jing-Kun, GAO Xiang, WANG Cheng, WANG Xiang-Nan

(School of Metallurgy, Northeastern University, Shenyang 110819, China)

Received:2016-12-22 Revised:2017-02-23 Published:2017-10-20 Online:2017-09-21
About author:ZHANG Xiao-Fang. E-mail: xfzhang2009@163.com
Supported by:
National Natural Science Foundation of China (51374055;52174059)

摘要/Abstract

摘要：

采用固相合成法制备了La_0.8Sr_0.2(Ga_0.8Mg_0.2)_0.1Fe_0.9O_3-_δ(LSGMF)混合导体和La_0.8Sr_0.2Ga_0.8Mg_0.2O_3-_δ(LSGM)固体电解质, 利用XRD、TGA、范德堡直流四探针法和热膨胀仪等对试样进行了分析。以LSGMF为致密扩散障碍层, 以LSGM为氧泵层, 采用共压共烧结法制备了极限电流型氧传感器, 利用SEM和EDS对LSGMF/LSGM陶瓷体横截面的微观形貌和成分进行了分析。结果表明: LSGMF具有菱方钙钛矿结构(R-3c空间群), 它在650℃失重速率最快, 其电导率随温度的升高而增大; 300~1000℃范围, LSGM与LSGMF的热膨胀系数分别为12.51×10^-6/℃和12.80×10^-6/℃。650~850℃范围, 氧传感器具有良好的极限电流平台, lgI_L(极限电流I_L)与1000/T呈线性关系, LSGMF中氧离子的扩散激活能为0.4008 eV。800℃、0.3mol%<x(O₂)<21.0mol%时, 极限电流I_L与氧含量x(O₂)间的关系为: I_L(mA)=10.285x(O₂)(mol%), R=0.9982。LSGMF和LSGM结合牢固, 未产生裂纹, EDS分析基本符合各化合物的化学计量比。

关键词: 氧传感器, 共压共烧结, 致密扩散障碍层, 极限电流

Abstract:

The La_0.8Sr_0.2(Ga_0.8Mg_0.2)_0.1Fe_0.9O_3-_δ(LSGMF) mixed conductor and La_0.8Sr_0.2Ga_0.8Mg_0.2O_3-_δ(LSGM) solid electrolyte were prepared by solid-state reaction and characterized by XRD, TGA, Van Der Pauw dc four-probe method, and thermal expansion measurement. A limiting current oxygen sensor with LSGMF as a dense diffusion barrier and LSGM as a solid electrolyte was prepared by a co-pressing and co-sintering method. The microstructure and composition of LSGMF/LSGM cross-section were analyzed by SEM and EDS. The results show that crystal structure of LSGMF is rhombohedral perovskite which belongs to R-3c space group. Its weight loss rate is the fastest at about 650℃. The electrical conductivity increases with the temperature increasing. The thermal expansion coefficients (TECs) of LSGM and LSGMF are 12.51×10^-6/℃ and 12.80×10^-6/℃ in the range of 300-1000℃, respectively. In the range of 650-850℃, the sensor exhibits an excellent limiting current plateau. lgI_L (limiting current) depends linearly on 1000/T, and the activation energy for oxide-ion diffusion in LSGMF is 0.4008 eV. The limiting current responses depend linearly on the oxygen concentration at 800℃ and 0.3mol% < x (O₂) < 21.0mol%, i.e., I_L (mA) = 10.285x (O₂) (mol%), R=0.9982. LSGMF and LSGM combines firmly without crack, and the mole ratio of their elements is basically in agreement with the stoichiometric of LSGMF and LSGM.

Key words: oxygen sensor, co-pressing and co-sintering, dense diffusion barrier layer, limiting current

中图分类号:

TQ174

张小芳, 刘涛, 金宏斌, 于景坤, 高翔, 王成, 王相南. 共压共烧法制备La_0.8Sr_0.2(Ga_0.8Mg_0.2)_0.1Fe_0.9O_3-_δ致密扩散障碍层极限电流型氧传感器[J]. 无机材料学报, 2017, 32(10): 1089-1094.

ZHANG Xiao-Fang, LIU Tao, JIN Hong-Bin, YU Jing-Kun, GAO Xiang, WANG Cheng, WANG Xiang-Nan. La_0.8Sr_0.2(Ga_0.8Mg_0.2)_0.1Fe_0.9O_3-_δ Dense Diffusion Barrier Limiting Current Oxygen Sensor Prepared by Co-pressing and Co-sintering Method[J]. Journal of Inorganic Materials, 2017, 32(10): 1089-1094.

图/表 8

图1 LSGMF和LSGM的XRD图谱

Fig. 1 XRD patterns of LSGMF and LSGM

图2 LSGMF的TG和DTG曲线

Fig. 2 TG and DTG curves of LSGMF

图3 LSGMF总电导率的Arrhenius曲线

Fig. 3 Arrhenius plot of total conductivity of LSGMF

图4 LSGM与LSGMF的热膨胀曲线

Fig. 4 Thermal expansion curves of LSGM and LSGMF

图5 不同温度下氧传感器的I-V曲线

Fig. 5 I-V curves of oxygen sensor at different temperatures

图6 不同氧含量下氧传感器的I-V曲线

Fig. 6 I-V curves of oxygen sensor with different oxygen contents

图7 LSGMF/LSGM截面的SEM照片(a)和区域A/B的EDS分析结果(b)和(c)

Fig. 7 SEM image(a) and EDS analysis of Area A/B for LSGMF/LSGM interface

图8 LSGMF/LSGM截面的SEM-EDS面扫描分析结果

Fig. 8 SEM-EDS plane scan analysis of LSGMF/LSGM interface

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共压共烧法制备La_0.8Sr_0.2(Ga_0.8Mg_0.2)_0.1Fe_0.9O_3-_δ致密扩散障碍层极限电流型氧传感器

La_0.8Sr_0.2(Ga_0.8Mg_0.2)_0.1Fe_0.9O_3-_δ Dense Diffusion Barrier Limiting Current Oxygen Sensor Prepared by Co-pressing and Co-sintering Method

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